Room-Temperature High-Performance Photodetector and Phototransistor Based on PdSe2/ZnIn2S4 Alloy Heterojunctions.

Various semiconductor devices have been developed based on 2D heterojunction materials owing to their distinctive optoelectronic properties. However, to achieve efficient charge transfer at their interface remains a major challenge. Herein, an alloy heterojunction concept is proposed. The sulfur vacancies in ZnIn2S4 are filled with selenium atoms of PdSe2. This chemically bonded heterojunction can significantly enhance the separation of photocarriers, providing notable advantages in the field of photoelectric conversion. As a demonstration, a two-terminal photodetector based on the PdSe2/ZnIn2S4 heterojunction materials is fabricated. The photodetector exhibits stable operation in ambient conditions, showcasing superior performance in terms of large photocurrent, high responsivity (48.8 mA W-1) and detectivity (1.98 × 1011 Jones). To further validate the excellent optoelectronic performance of the heterojunction, a tri-terminal phototransistor is also fabricated. Benefiting from gate voltage modulation, the photocurrent is amplified to milliampere level, and the responsivity is increased to 229.14 mA W-1. These findings collectively demonstrate the significant potential of the chemically bonded PdSe2/ZnIn2S4 alloy heterojunction for future optoelectronic applications.

Sb3+/Sm3+ Codoped Cs2NaScCl6 All-Inorganic Double Perovskite: Blue Emission of Self-Trapped Excitons and Red-Emission via Energy Transfer.

The lead-free halide perovskites possess nontoxicity and excellent chemical stability, whereas relatively weak luminescence intensity limits their potential in practical applications. Therefore, strengthening the luminescence intensity and expanding application fields are urgent tasks for the development of lead-free halide perovskites. In this paper, antimony-doped Cs2NaScCl6 crystals synthesized by a solvothermal method emit bright, deep blue photoluminescence at 447 nm. The photoluminescence (PL), photoluminescence excitation (PLE), and absorption spectra demonstrate that Sb3+ doping effectively activate the intrinsic "dark self-trapped exciton (STE)," leading to an impressive photoluminescence quantum yield (PLQY) value of 78.31% for 1% Sb3+ doping. Furthermore, the luminescence intensity remains above 92% compared with the fresh sample without secondary phases detected even after 90 days under environmental conditions. To expand the emission spectra, rare-earth Sm3+ is further incorporated into Cs2NaScCl6:1% Sb3+ crystals. The results show that Sb ions not only enhance intrinsic STE luminescence but also serve as sensitizers to boost the red-light emission of Sm3+, leading to a significant 500-fold increase in red emission intensity. Finally, the PLQY reaches a stunning 86.78%. These findings provide valuable insights in the design of Sb ion-doped lead-free double perovskites, broadening the application fields in various optoelectronic devices.

Modulating the afterglow time of Mn2+ doped double perovskites by size tuning and its applications in dynamic information display.

Mn2+ doped lead-free double perovskites are emerging afterglow materials that can avoid the usage of rare earth ions. However, the regulation of the afterglow time is still a challenge. In this work, the Mn doped Cs2Na0.2Ag0.8InCl6 crystals with afterglow emission at about 600 nm are synthesized by a solvothermal method. Then, the Mn2+ doped double perovskite crystals are crushed into different sizes. As the size decreases from 1.7 mm to 0.075 mm, the afterglow time decreases from 2070 s to 196 s. Steady-state photoluminescence (PL) spectra, time resolved PL, thermoluminescence (TL) reveal the afterglow time monotonously decreases due to the enhanced nonradiative surface trapping. The modulation on afterglow time will greatly promote their applications in various fields, such as bioimaging, sensing, encryption, and anti-counterfeiting. As a proof of concept, dynamic display of information is realized based on different afterglow times.

Co-multiplexing spectral and temporal dimensions based on luminescent materials.

Optical multiplexing is a pivotal technique for augmenting the capacity of optical data storage (ODS) and increasing the security of anti-counterfeiting. However, due to the dearth of appropriate storage media, optical multiplexing is generally restricted to a single dimension, thus curtailing the encoding capacity. Herein, the co-multiplexing spectral and temporal dimensions are proposed for optical encoding based on photoluminescence (PL) and persistent-luminescence (PersL) at four different wavelengths. Each emission color comprises four luminescence modes. The further multiplexing of four wavelengths leads to the maximum encoding capacity of 8 bits at each pixel. The wavelength difference between adjacent peaks is larger than 50 nm. The well-separated emission wavelengths significantly lower the requirements for high-resolution spectrometers. Moreover, the information is unable to be decoded until both PL and PersL spectra are collected, suggesting a substantial improvement in information security and the security level of anti-counterfeiting.

A droplet friction/solar-thermal hybrid power generation device for energy harvesting in both rainy and sunny weathers.

Photovoltaic device is highly dependent on the weather, which is completely ineffective on rainy days. Therefore, it is very significant to design an all-weather power generation system that can utilize a variety of natural energy. This work develops a water droplet friction power generation (WDFG)/solar-thermal power generation (STG) hybrid system. The WDFG consists of two metal electrodes and a candle soot/polymer composite film, which also can be regarded as a capacitor. Thus, the capacitor coupled power generation (C-WDFG) device can achieve a sustainable and stable direct-current (DC) output under continuous dripping without external conversion circuits. A single device can produce an open-circuit voltage of ca.0.52 V and a short-circuit current of ca.0.06 mA, which can be further scaled up through series or parallel connection to drive commercial electronics. Moreover, we demonstrate that the C-WDFG is highly compatible with the thermoelectric device. The excellent photothermal performance of soot/polymer composite film can efficiently convert solar into heat, which is then converted to electricity by the thermoelectric device. Therefore, this C-WDFG/STG hybrid system can work in both rainy and sunny days.

Snapshot multi-frame parallel spectral holographic microscopy based on a reconfigurable optical comb.

We present a snapshot multi-frame parallel holographic microscopy system through a reconfigurable optical comb source, which consists of a digital micromirror device (DMD) based spectrum filter system and a spectroscopic Michelson interferometric system. The proposed system allows arbitrarily tuning comb spacing and comb number, and the capturing of multi-frame images without overlap in one exposure. As a result, high-quality spectral holograms can be obtained with less acquisition time. The performance of the system is detailed in the experiment and 45-wavelengths holographic imaging for perovskite micro-platelets is conducted, which proves the system has the ability to realize high-performance four-dimensional (4D) imaging.

Structural characterizations on the degradation of 2D organic-inorganic hybrid perovskites and its enlightenment to improved stability.

Despite the demonstrated high-efficiency of solar cells and light-emitting devices based on two-dimensional (2D) perovskites, intrinsic stability of the 2D perovskites is yet far from satisfactory. In this work, we find the 2D (BA)2PbI4perovskite crystals rapidly degrade in the ambient conditions and the photoluminescence (PL) nearly completely quenches in 6 d. Moreover, the PL shoulder band due to defects and absorption band of PbI2gradually rise during degradation, suggesting the precipitation of PbI2. Besides, rod structures are observed in the degraded crystals, which are attributed to the formation of one-dimensional (1D) (BA)3PbI5perovskites. And the degradation can be largely retarded by decreasing the humidity during storage. Therefore, a chemical reaction for the degradation of (BA)2PbI4is proposed, revealing the interactions between water molecules and undercoordinated defects are very critical for understanding the degradation. Enlightened by these findings, dimethyl itaconate (DI) treatment is developed to passivate the defects and block the intrusion of moisture to improve the stability of the (BA)2PbI4. After storage in the ambient environment for 16 d, the DI treated (BA)2PbI4only shows a slight surface degradation without formation of any nanorod-like structures, and the PL intensity retains about 70%. Therefore, our systematic study provides a comprehensive understanding on the degradation dynamics of 2D perovskites, which will promote future development of intrinsically stable 2D perovskites.

Fluorescent dynamics of CsPbBr3 nanocrystals in polar solvents: a potential sensor for polarity.

During synthesis, device processes, and applications of perovskite nanocrystals (NCs), there are usually inevitable interactions between perovskite NCs and polar solvents. To elaborately control the properties of perovskite NCs, investigating the effects of solvent polarity on perovskite NCs is thus highly important. Herein, fluorescent variations induced by different solvents into CsPbBr3 NCs solution are systematically studied. In this report, it is found that when CsPbBr3 NCs are treated with polar solvents, the fluorescence intensity decreases with a general redshift of fluorescence peak position. Moreover, the fluorescence quenching and peak position shift amplitude monotonously increase with the solvent polarity. Absorption spectra and fluorescent lifetime suggest that, with addition of polar solvents, the surface of NCs are destroyed and defect states are generated, leading to the fluorescent variations. Besides, dielectric constant of the solvent also increases with polarity, which may weaken the quantum confinement effect and decrease the exciton binding energy. We find the fluorescence may slightly blue shift if the emission of free carrier is strong enough with certain solvents, such as dimethylsulfoxide (DMSO). We also find the fluorescence intensity generally deceases to a stable state in 2 min, indicating quick interactions between CsPbBr3 NCs and solvents. However, water continuously quenches the fluorescence of CsPbBr3 NCs up to 72 h due to the poor miscibility between water and n-hexane. This work not only provides a comprehensive understanding on the fluorescent dynamics of CsPbBr3 NCs in polar solvents but also affords a potential fluorescent indicator for solvent polarity.

Photoluminescent Spectral Broadening of Lead Halide Perovskite Nanocrystals Investigated by Emission Wavelength Dependent Lifetime.

Despite intensive efforts, the fluorescence of perovskite nanocrystals (NCs) still suffers from a poor color purity, which limits the applications in light emitting and multicolor display. A deep understanding on the fundamental of the photoluminescent (PL) spectral broadening is thus of great significance. Herein, the PL decay curves of the CsPbClxBr3-x NCs are monitored at different wavelengths covering the entire PL band. Moreover, energy relaxation time τ and radiative recombination time ß are obtained by numerical fittings. The dependences of τ and 1/ß on the detection wavelength agree well with the steady-state PL spectrum, indicating the observed PL broadening is an intrinsic effect due to the resonance and off-resonance exciton radiative recombination processes. This work not only provides a new analysis method for time-resolved PL spectra of perovskites, but also gains a deep insight into the spectral broadening of the lead halide perovskite NCs.

Investigation of energy transfer mechanisms in rare-earth doped amorphous silica films embedded with tin oxide nanocrystals.

Three different types of rare earth (RE3+) ions-doped silica thin films are fabricated by a soft chemistry-based method. By introducing tin oxide (SnO2) nanocrystals with larger cross-sections as sensitizers, the characteristic emission intensity of RE3+ ions in amorphous silica thin films can be enhanced by more than two orders of magnitude via the energy transfer process. The possible energy transfer processes under different local environment are revealed by using Eu3+ ions as an optical probe. Quantitative studies of PL decay lifetime and temperature-dependence PL spectra suggest that the partial incorporation of RE3+ ions into SnO2 sites gives rises to the change of crystal-field symmetry and the significant enhancement of energy transfer efficiency. Further, typical analytical energy dispersive X-ray spectroscopy (EDS) mapping results prove that part of Eu3+ ions doped into the SnO2 sites after annealing at 1000 °C. We anticipate that our results would shed light on the future research on the energy transfer mechanisms under different local structures of RE3+ ions.

Porous reduced graphene oxide/nickel foam for highly efficient solar steam generation.

Solar-driven water evaporation is considered to be an effective method for seawater desalination and wastewater purification. Here, we report a novel solar steam generation (SSG) system based on reduced graphene oxide (rGO)/nickel foam. Porous rGO foam acting as a photothermal conversion layer is fabricated by coating the rGO microsheets on the metallic nickel foam. The porous structure shows a rough surface, which can improve the harvest of light by scattering effect. On the other hand, the porous structure ensures the rapid flow of steam in the evaporation process. This SSG system based on rGO/nickel foam converts the absorbed solar energy into heat energy at the water-air interface and can effectively evaporate (∼83.4%) under low irradiation of 1 sun (1 kw m-2). The system shows great potential for the practical applications of water treatment at large-scale because of the high efficiency, simple preparation method and low cost.

Copper nanoparticles with near-unity, omnidirectional, and broadband optical absorption for highly efficient solar steam generation.

Solar steam generation provides a renewable and environmentally friendly approach to solve the water shortage issue. The pursuit of efficient, stable, and cheap photothermal agents is thus of great significance. In this work, Cu nanoparticles (NPs) fabricated simply by a substitution reaction, exhibit a near-unity (∼97.7%) light absorption, covering a broad incident angle and wavelength range (200-1300 nm). Thereby, a high photothermal conversion efficiency of 93% is achieved. The excellent photothermal performance offers a unique opportunity for the development of solar steam generation. By coating the Cu NPs on a cellulose membrane, a solar steam generation efficiency up to 73% is acquired at a low irradiation power density of 2 kW m-2 (1 kW m-2 = 1 sun). Moreover, the Cu NPs are recyclable with the high stability being resistant to heat, photoirradiation and corrosion of brine.

Ultraviolet Photoluminescence of Carbon Nanospheres and its Surface Plasmon-Induced Enhancement.

Ultraviolet (UV) light can be used in versatile applications ranging from photoelectronic devices to biomedical imaging. In the development of new UV light sources, in this study, stable UV emission at ≈350 nm is unprecedentedly obtained from carbon nanospheres (CNSs). The origin of the UV fluorescence is comprehensively investigated via various characterization methods, including Raman and Fourier transform infrared analyses, with comparison to the visible emission of carbon nanodots. Based on the density functional calculations, the UV fluorescence is assigned to the carbon nanostructures bonded to bridging O atoms and dangling -OH groups. Moreover, a twofold enhancement in the UV emission is acquired for Au-carbon core-shell nanospheres (Au-CNSs). This remarkable modification of the UV emission is primarily ascribed to charge transfer between the CNSs and the Au surface.

Hydrogenated TiO2 nanotube photonic crystals for enhanced photoelectrochemical water splitting.

We report the design, fabrication and characterization of novel TiO2 nanotube photonic crystals with a crystalline core/disordered shell structure as well as substantial oxygen vacancies for photoelectrochemical (PEC) water splitting. The novel TiO2 nanotube photonic crystals are fabricated by annealing of anodized TiO2 nanotube photonic crystals in hydrogen atmosphere at various temperatures. The optimized novel TiO2 nanotube photonic crystals produce a maximal photocurrent density of 2.2 mA cm-2 at 0.22 V versus Ag/AgCl, which is two times higher that of the TiO2 nanotube photonic crystals annealed in air. Such significant PEC performance improvement can be ascribed to synergistic effects of the disordered surface layer and oxygen vacancies. The reduced band gap owing to the disordered surface layer and localized states induced by oxygen vacancies can enhance the efficient utilization of visible light. In addition, the disordered surface layer and substantial oxygen vacancies can promote the efficiency for separation and transport of the photogenerated carriers. This work may open up new opportunities for the design and construction of the high efficient and low-cost PEC water splitting system.

Bright, stable, and tunable solid-state luminescence of carbon nanodot organogels.

Despite the sustained enthusiastic interest in fluorescent carbon nanodots (FCNDs), it is still challenging to achieve bright and widely tunable solid-state luminescence. Herein, organogels embedded with FCNDs were simply synthesized via a one-pot pyrolysis method. Subsequently, the excitation of a single ultraviolet (UV) excitation line results in tunable solid-state luminescence ranging from blue to red with quantum yields (QYs) >14%. In this study, N and S elements were co-doped to regulate the aggregation of FCNDs, which consequently modulated the Stokes shift of the photoluminescence (PL) by managing the degree of photon reabsorption. Notably, without compact aggregations, the dispersions of FCNDs in the organogel matrix indeed render bright fluorescence, which results from the suppression of excessive photon reabsorption and nonradiative resonant energy transfer (NRET).

Photoluminescence of Diphenylalanine Peptide Nano/Microstructures: From Mechanisms to Applications.

Diphenylalanine (Phe-Phe, FF) molecules, which can self-assemble into highly ordered nano/microstructures, have increasingly aroused intense interests due to their special optical properties. In this review, recent advances in photoluminescence (PL) of supramolecular architectures of FF-based peptide and the underlying mechanisms are highlighted. Mainly deep ultraviolet emission at around 285 nm and/or blue emission at ≈450 nm are observed in various FF peptide structures and its derivatives, which are primarily interpreted by quantum confinement effects, shallow radiative traps, and electron delocalization via hydrogen bonds in ß-sheet structures. Furthermore, current applications of such fluorescent peptide nano/microstructures are also reviewed here, e.g., probing the number of water molecules confined in FF, temperature sensing, and visualization of deep ultraviolet beam. Yet, the PL mechanism is still under fierce debate and the application based on fluorescence is constantly under exploration. Thus, this review is endeavored to boost future explorations on the PL of the bioinspired FF peptide nano/microstructures.

Research Progress on Rashba Effect in Two-Dimensional Organic-Inorganic Hybrid Lead Halide Perovskites.

The Rashba effect appears in the semiconductors with an inversion-asymmetric structure and strong spin-orbit coupling, which splits the spin-degenerated band into two sub-bands with opposite spin states. The Rashba effect can not only be used to regulate carrier relaxations, thereby improving the performance of photoelectric devices, but also used to expand the applications of semiconductors in spintronics. In this mini-review, recent research progress on the Rashba effect of two-dimensional (2D) organic-inorganic hybrid perovskites is summarized. The origin and magnitude of Rashba spin splitting, layer-dependent Rashba band splitting of 2D perovskites, the Rashba effect in 2D perovskite quantum dots, a 2D/3D perovskite composite, and 2D-perovskites-based van der Waals heterostructures are discussed. Moreover, applications of the 2D Rashba effect in circularly polarized light detection are reviewed. Finally, future research to modulate the Rashba strength in 2D perovskites is prospected, which is conceived to promote the optoelectronic and spintronic applications of 2D perovskites.

Ultrasensitive Detection of Matrix Metalloproteinase 2 Activity Using a Ratiometric Surface-Enhanced Raman Scattering Nanosensor with a Core-Satellite Structure.

Matrix metalloproteinase 2 (MMP-2) has been considered a promising molecular biomarker for cancer diagnosis due to its related dysregulation. In this work, a core-satellite structure-powered ratiometric surface-enhanced Raman scattering (SERS) nanosensor with high sensitivity and specificity to MMP-2 was developed. The SERS nanosensor was composed of a magnetic bead encapsulated within a 5,5'-dithiobis(2-nitrobenzoic acid) (DTNB)-labeled gold shell as the capture core and a 4-mercaptobenzonitrile (MBN)-encoded silver nanoparticle as the signal satellite, which were connected through a peptide substrate of MMP-2. MMP-2-triggered cleavage of peptides from the core surface resulted in a decrease of the SERS intensity of MBN. Since the SERS intensity of DTNB was used as an internal standard, the reliable and sensitive quantification of MMP-2 activity would be realized by the ratiometric SERS signal, with a limit of detection as low as 2.067 ng/mL and a dynamic range from 5 to 100 ng/mL. Importantly, the nanosensor enabled a precise determination of MMP-2 activity in tumor cell secretions, which may provide an avenue for early diagnosis and classification of malignant tumors.

Advanced Optical Information Encryption Enabled by Polychromatic and Stimuli-Responsive Luminescence of Sb-Doped Double Perovskites.

The smart materials with multi-color and stimuli-responsive luminescence are very promising for next generation of optical information encryption and anti-counterfeiting, but these materials are still scarce. Herein, a multi-level information encryption strategy is developed based on the polychromatic emission of Sb-doped double perovskite powders (SDPPs). Cs2NaInCl6:Sb, Cs2KInCl6:Sb, and Cs2AgInCl6:Sb synthesized through coprecipitation methods exhibit broadband emissions with bright blue, cyan, and orange colors, respectively. The information transmitted by specific SDPP is encrypted when different SDPPs are mixed. The confidential information can be decrypted by selecting the corresponding narrowband filter. Then, an encrypted quick response (QR) code with improved security is demonstrated based on this multi-channel selection strategy. Moreover, the three types of SDPPs exhibit three different water-triggered luminescence switching behaviors. The confidential information represented by Cs2NaInCl6:Sb can be erased/recovered through a simple water spray/drying. Whereas, the information collected from the green channel is permanently erased by moisture, which fundamentally avoids information leakage. Therefore, different encryption schemes can be designed to meet a variety of encryption requirements. The multicolor and stimuli-responsive luminescence greatly enrich the flexibility of optical information encryption, which leaps the level of security and confidentiality.

Perovskite Quantum Heterostructure Constructed by Halide Mixing between a Single CsPbI3 Nanocrystal and an Individual CsPbBr3 Microplate.

Ion migration is significantly enhanced in lead-halide perovskites with a soft crystal lattice, which can promote the formation of a heterogeneous interface between two such materials with different halide-anion compositions. Here we have deposited a single CsPbI3 nanocrystal (NC) on top of an individual CsPbBr3 microplate to create a mixed-halide CsPbBrxI3-x (0 < x < 3) NC by means of the anion exchange process. The formation of a CsPbBrxI3-x/CsPbBr3 heterostructure is confirmed by the much-enlarged geometric volume of the CsPbBrxI3-x NC as compared to the original CsPbI3 one, as well as by its capability of receiving photogenerated excitons from the CsPbBr3 microplate with a larger bandgap energy. The quantum nature of this heterostructure is reflected from single-photon emission of the composing CsPbBrxI3-x NC, which can also be bulk-like during phase segregation to demonstrate a red shift in the photoluminescence peak that is opposite to the common trend observed in smaller-sized mixed-halide NCs.